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SummaryThe primary purpose of the work reported here is to analyze the potential effect of the release of technetium (Tc) from metal inclusions in bulk vitrification (BV) waste packages once they are placed in the Integrated Disposal Facility (IDF). As part of the strategy for immobilizing waste from the underground tanks at Hanford, selected wastes will be immobilized using BV. During analyses of the glass produced in engineering-scale tests, metal inclusions were found in the glass product. This report contains the results from experiments designed to quantify the corrosion rates of metal inclusions found in the glass product from Test ES-32B (AMEC 2005) and simulations designed to compare the rate of Tc release from the metal inclusions to the release of Tc from glass produced with the BV process. Due to the probability of oxidizing conditions surrounding the waste packages in the IDF, in the simulations the Tc in the metal inclusions and the glass is conservatively assumed to be released congruently as soluble TcO 4 -. The experimental results and modeling calculations (Bacon and McGrail 2005) show that the metal corrosion rate will, under all conceivable conditions at the IDF, be dominated by the presence of the passivating layer and corrosion products on the metal particles. As a result, the release of Tc from the metal particles at the surfaces of fractures in the glass releases at a rate similar to the Tc present as a soluble salt (McGrail et al. 2003;Pierce et al. 2005). The release of the remaining Tc in the metal is controlled by the dissolution of the glass matrix.The dissolution kinetics of iron [Fe(0)] was quantified under conditions of constant dissolved O 2 [O 2 (aq)] and in solutions that minimized the formation of a passive film on the metal surface. These tests were performed to determine the forward reaction rate for the metal inclusions in the BV glass. Single-pass flow through (SPFT) tests were conducted over the pH(23°C) range from 7.0 to 12.0 and temperature range from 23°C to 90°C. The presence of EDTA minimized the formation of a passive film and Fe-bearing secondary phase(s) during testing allowing us to determine the forward dissolution rate. These results indicate that the corrosion of Fe(0) is relatively insensitive to pH and temperature and the forward rate is 3 to 4 orders of magnitude higher than when a passive film and corrosion products are present. Tests conducted with Amasteel (a low carbon steel non-radioactive surrogate) and ES-32B metal indicated that the forward dissolution rates for both metals were similar, if not identical. In other words, the presence of P and 99 Tc in the ES-32B metal appeared to have little effect on the forward dissolution rate. These results indicate that the corrosion rate of the ES-32B metal at repository relevant conditions was not significantly less than the surrogate metal. Because the effects of temperature (E a = 15 ±5 kJ/mol at pH(23°C) = 9.0 based on Fe release from ES-32B metal) and solution pH (η = -0.13 ±0.02 at 70°C based on Fe releas...
SummaryThe primary purpose of the work reported here is to analyze the potential effect of the release of technetium (Tc) from metal inclusions in bulk vitrification (BV) waste packages once they are placed in the Integrated Disposal Facility (IDF). As part of the strategy for immobilizing waste from the underground tanks at Hanford, selected wastes will be immobilized using BV. During analyses of the glass produced in engineering-scale tests, metal inclusions were found in the glass product. This report contains the results from experiments designed to quantify the corrosion rates of metal inclusions found in the glass product from Test ES-32B (AMEC 2005) and simulations designed to compare the rate of Tc release from the metal inclusions to the release of Tc from glass produced with the BV process. Due to the probability of oxidizing conditions surrounding the waste packages in the IDF, in the simulations the Tc in the metal inclusions and the glass is conservatively assumed to be released congruently as soluble TcO 4 -. The experimental results and modeling calculations (Bacon and McGrail 2005) show that the metal corrosion rate will, under all conceivable conditions at the IDF, be dominated by the presence of the passivating layer and corrosion products on the metal particles. As a result, the release of Tc from the metal particles at the surfaces of fractures in the glass releases at a rate similar to the Tc present as a soluble salt (McGrail et al. 2003;Pierce et al. 2005). The release of the remaining Tc in the metal is controlled by the dissolution of the glass matrix.The dissolution kinetics of iron [Fe(0)] was quantified under conditions of constant dissolved O 2 [O 2 (aq)] and in solutions that minimized the formation of a passive film on the metal surface. These tests were performed to determine the forward reaction rate for the metal inclusions in the BV glass. Single-pass flow through (SPFT) tests were conducted over the pH(23°C) range from 7.0 to 12.0 and temperature range from 23°C to 90°C. The presence of EDTA minimized the formation of a passive film and Fe-bearing secondary phase(s) during testing allowing us to determine the forward dissolution rate. These results indicate that the corrosion of Fe(0) is relatively insensitive to pH and temperature and the forward rate is 3 to 4 orders of magnitude higher than when a passive film and corrosion products are present. Tests conducted with Amasteel (a low carbon steel non-radioactive surrogate) and ES-32B metal indicated that the forward dissolution rates for both metals were similar, if not identical. In other words, the presence of P and 99 Tc in the ES-32B metal appeared to have little effect on the forward dissolution rate. These results indicate that the corrosion rate of the ES-32B metal at repository relevant conditions was not significantly less than the surrogate metal. Because the effects of temperature (E a = 15 ±5 kJ/mol at pH(23°C) = 9.0 based on Fe release from ES-32B metal) and solution pH (η = -0.13 ±0.02 at 70°C based on Fe releas...
Evapotranspiration (ET) surface barriers store infiltrated precipitation during the recharge period and release the stored water to the atmosphere via ET. The primary purpose of a surface barrier is to reduce or eliminate drainage to the underlying waste zone. The objective of this study is to analyze the spatial and temporal dynamics of soil moisture within an ET surface barrier based on observed and simulated data. This study characterizes the water movement processes using contour plots of soil moisture content and flux rate in the depth‐time domain. Zero‐flux planes (ZFPs) divide the depth‐time domain into stored water, ET, and drainage zones. Some flow dynamics (e.g., flow rate and direction) that were not observed in the field were elaborated with simulation results to identify the depth of the recharge front of infiltrated water, the release front of stored water, and the bottom of the ET zone. The ET‐drainage divide marks the bottom of the ET zone and the top of the drainage zone. The results showed that the temporal analysis of soil moisture storage could indicate the degree of usage of the storage capacity of a surface barrier. The spatial‐temporal analyses of soil moisture content and flux rate can characterize the durations of the recharge/release processes and the depth of the stored water. Quantification of these processes and related zones provides beneficial understanding of the state and dynamics of soil moisture for a range of weather and vegetation conditions and is useful in optimizing the design of an ET surface barrier.
Current plans for treatment and disposal of immobilized low-activity waste (ILAW) from Hanford's underground waste storage tanks include vitrification and storage of the glass waste form in a near-surface disposal facility. This Integrated Disposal Facility (IDF) is located in the 200 East Area of the Hanford Central Plateau. Performance assessment (PA) of the IDF requires numerical modeling of subsurface flow and reactive transport processes over very long periods (thousands of years). The models used to predict facility performance require parameters describing various physical, hydraulic, and transport properties. This report provides updated estimates of physical, hydraulic, and transport properties and parameters for both near-and far-field materials, intended for use in future IDF PA modeling efforts. Previous work on physical and hydraulic property characterization for earlier IDF PA analyses is reviewed and summarized. For near-field materials, portions of this document and parameter estimates are taken from an earlier data package. For far-field materials, a critical review is provided of methodologies used in previous data packages. Alternative methods are described and associated parameters are provided. For far-field materials, consisting of both sand-and gravel-dominated facies underlying the IDF, a particular model has been used in previous PA modeling efforts to represent the saturation-dependent anisotropy of unsaturated hydraulic conductivity. We recommend that this model be replaced with a more recent and general tensorial pore-connectivity-tortuosity (TCT) model for saturation-dependent anisotropy. Simulation results from both the TCT and the earlier anisotropy model have been compared with observed data from a controlled vadose zone field injection experiment performed just south of the 200 East Area. The TCT model was shown to predict observed flow behavior at this site as well as or better than the model used in previous PA efforts, and with many fewer added model parameters (one versus eight). Recommended parameter estimates for the TCT model are presented. Previous estimates of dispersivities for vadose zone sediments were based on stochastic theory developed for saturated aquifer materials. An extensive literature review is presented that suggests these estimates may not be appropriate for unsaturated conditions. An alternative approach based on more fundamental physical property information is described and updated parameter estimates are presented.
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